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Boosting diethylamine selective oxidation over CuO/ZSM-5 catalyst by CeO2 modification

Journal 2023 · IF 7.4 · 发表于 2023 年 2 月 22 日
作者: Lin-Cong He,Hua-Hui Xu,Xing-Yue Leng,Ling-Yun Jin,Ai-Ping Jia,Meng-Fei Luo,Jian Chen
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摘要

Selective catalytic oxidation of nitrogen containing volatile organic compounds (NVOCs) is very meaningful but still remains big challenge because it is very difficult to balance the oxidation activity and N 2 selectivity of available catalysts. In order to develop excellent catalysts with high N 2 selectivity in wide temperature window ( △T ) during NVOCs oxidation, CeO 2 modified CuO/ZSM-5 catalysts with different CeO 2 addition order were prepared for diethylamine (DEA) oxidation. Detailed characterizations of catalysts such as XRD, XPS, H 2 -TPR and NH 3 -TPD were conducted, it is found that addition of CeO 2 obviously changes the geometrical and electronic states of CuO active sites in the catalyst, and CeO 2 addition order affects the Ce 3+ ratio on the catalyst surface. Promotion of CeO 2 species enables the generation of more highly active Cu species (Cu + species and finely dispersed CuO clusters) for DEA oxidation; and synergistic catalysis of the Ce 3+ species, active Cu species and acid sites in ZSM-5 leads to the high N 2 selectivity in wide temperature window ( △T ). Compared to the CeO 2 /CuO/ZSM-5 and CuO-CeO 2 /ZSM-5 catalysts, the CuO/CeO 2 /ZSM-5 catalyst exhibits moderate high oxidation activity with T 99 of 230 °C and the widest △T of 150 °C for high N 2 selectivity. Our primary results in this work provide the efficient strategy for improving catalyst employed for NVOCs selective oxidation.

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